The simple algebraic and geometric properties of naturally reductive metrics make them useful as examples in the study of homogeneous Riemannian manifolds. (See for example [2], [3], [15]). The existence and abundance of naturally reductive left-invariant metrics on a Lie group G or homogeneous space G/L reflect the structure of G itself. Such metrics abound on compact groups, exist but are more restricted on noncompact semisimple groups, and are relatively rare on solvable groups. The goals of this paper are(i) to study all naturally reductive homogeneous spaces of G when G is either semisimple of noncompact type or nilpotent and(ii) to give necessary conditions on a Riemannian homogeneous space of an arbitrary Lie group G in order that the metric be naturally reductive with respect to some transitive subgroup of G.